Location and orientation of the N,N-diisopropylethylamine template molecule in the AlPO4-18 framework by X-ray synchrotron diffraction and molecular modelling

引用本文: Christiana Zenonos, Dewi W. Lewis, Gopinathan Sankar. Location and orientation of the N,N-diisopropylethylamine template molecule in the AlPO₄-18 framework by X-ray synchrotron diffraction and molecular modelling[J]. 催化学报, 2015, 36(6): 874-879. doi: 10.1016/S1872-2067(14)60306-5 shu

Citation: Christiana Zenonos, Dewi W. Lewis, Gopinathan Sankar. Location and orientation of the N,N-diisopropylethylamine template molecule in the AlPO₄-18 framework by X-ray synchrotron diffraction and molecular modelling[J]. Chinese Journal of Catalysis, 2015, 36(6): 874-879. doi: 10.1016/S1872-2067(14)60306-5 shu

Location and orientation of the N,N-diisopropylethylamine template molecule in the AlPO₄-18 framework by X-ray synchrotron diffraction and molecular modelling

通讯作者: Gopinathan Sankar,Tel: +44-2076794664; E-mail: g.sankar@ucl.ac.uk

摘要: Phase pure AlPO₄ with the AlPO₄-18 (AEI) structure was synthesised using N,N- diisopropylethylamine as a template. Using a combination of X-ray powder diffraction and computational methods, the location and orientation of the N,N-diisopropylethylamine molecules inside the cages of the AEI structure were determined. Thermogravimetric analysis confirmed that the number of template molecules per unit cell was consistent with the diffraction study. We unequivocally show that only one template molecule is present in each cage of the crystalline AEI material. Our work demonstrates that a combined approach enables accurate structure resolution of such complex materials.

关键词:

English

Location and orientation of the N,N-diisopropylethylamine template molecule in the AlPO₄-18 framework by X-ray synchrotron diffraction and molecular modelling

1.
Department of Chemistry, University College London, 20 Gordon Street, London WC1H 0AJ, United Kingdom

Corresponding author: Gopinathan Sankar,Tel: +44-2076794664; E-mail: g.sankar@ucl.ac.uk

Received Date: 18 December 2014
Available Online: 20 June 2015

Abstract: Phase pure AlPO₄ with the AlPO₄-18 (AEI) structure was synthesised using N,N- diisopropylethylamine as a template. Using a combination of X-ray powder diffraction and computational methods, the location and orientation of the N,N-diisopropylethylamine molecules inside the cages of the AEI structure were determined. Thermogravimetric analysis confirmed that the number of template molecules per unit cell was consistent with the diffraction study. We unequivocally show that only one template molecule is present in each cage of the crystalline AEI material. Our work demonstrates that a combined approach enables accurate structure resolution of such complex materials.

Key words:

1. [1] Flanigen E M, Lok B M, Patton R L, Wilson S T. Pure Appl Chem, 1986, 58: 1351[1] Flanigen E M, Lok B M, Patton R L, Wilson S T. Pure Appl Chem, 1986, 58: 1351
2. [2] Wilson S T, Lok B M, Messina C A, Cannan T R, Flanigen E M. J Am Chem Soc, 1982, 104: 1146[2] Wilson S T, Lok B M, Messina C A, Cannan T R, Flanigen E M. J Am Chem Soc, 1982, 104: 1146
3. [3] Wilson S T, Lok B M, Messina C A, Cannan T R, Flanigen E M. ACS Symp Ser, 1983, 218: 79[3] Wilson S T, Lok B M, Messina C A, Cannan T R, Flanigen E M. ACS Symp Ser, 1983, 218: 79
4. [4] Cheetham A K, Ferey G, Loiseau T. Angew Chem Int Ed, 1999, 38: 3268[4] Cheetham A K, Ferey G, Loiseau T. Angew Chem Int Ed, 1999, 38: 3268
5. [5] Cheetham A K, Rao C N R. MRS Bull, 2005, 30: 93[5] Cheetham A K, Rao C N R. MRS Bull, 2005, 30: 93
6. [6] Hartmann M, Elangovan S P. Adv Nanoporous Mater, 2009, 1: 237[6] Hartmann M, Elangovan S P. Adv Nanoporous Mater, 2009, 1: 237
7. [7] Li J Y, Yu J H, Xu R R. Proc Royal Soc A, 2012, 468: 1955[7] Li J Y, Yu J H, Xu R R. Proc Royal Soc A, 2012, 468: 1955
8. [8] Li J Y, Yu J H, Xu R R. Chin J Inorg Chem (李激扬, 于吉红, 徐如人. 无机化学学报), 2004, 20: 1[8] Li J Y, Yu J H, Xu R R. Chin J Inorg Chem (李激扬, 于吉红, 徐如人. 无机化学学报), 2004, 20: 1
9. [9] Simmen A, McCusker L B, Baerlocher C, Meier W M. Zeolites, 1991, 11: 654[9] Simmen A, McCusker L B, Baerlocher C, Meier W M. Zeolites, 1991, 11: 654
10. [10] Thomas J M, Raja R, Sankar G, Bell R G. Nature, 1999, 398: 227[10] Thomas J M, Raja R, Sankar G, Bell R G. Nature, 1999, 398: 227
11. [11] Thomas J M, Raja R, Sankar G, Bell R G. Acc Chem Res, 2001, 34: 191[11] Thomas J M, Raja R, Sankar G, Bell R G. Acc Chem Res, 2001, 34: 191
12. [12] Yu J H, Xu R R. Chem Soc Rev, 2006, 35: 593[12] Yu J H, Xu R R. Chem Soc Rev, 2006, 35: 593
13. [13] Barrett P A, Sankar G, Stephenson R, Catlow C R A, Thomas J M, Jones R H, Teat S J. Solid State Sci, 2006, 8: 337[13] Barrett P A, Sankar G, Stephenson R, Catlow C R A, Thomas J M, Jones R H, Teat S J. Solid State Sci, 2006, 8: 337
14. [14] Martinez-Franco R, Moliner M, Yun Y F, Sun J L, Wan W, Zou X D, Corma A. Proc Natl Acad Sci U S A, 2013, 110: 3749[14] Martinez-Franco R, Moliner M, Yun Y F, Sun J L, Wan W, Zou X D, Corma A. Proc Natl Acad Sci U S A, 2013, 110: 3749
15. [15] Stocker M. Microporous Mesoporous Mater, 1999, 29: 3[15] Stocker M. Microporous Mesoporous Mater, 1999, 29: 3
16. [16] Ma L, Cheng Y S, Cavataio G, McCabe R W, Fu L X, Li J H. Chem Eng J, 2013, 225: 323[16] Ma L, Cheng Y S, Cavataio G, McCabe R W, Fu L X, Li J H. Chem Eng J, 2013, 225: 323
17. [17] Mathisen K, Stockenhuber M, Nicholson D G. Phys Chem Chem Phys, 2009, 11: 5476[17] Mathisen K, Stockenhuber M, Nicholson D G. Phys Chem Chem Phys, 2009, 11: 5476
18. [18] Lewis D W, Catlow C R A, Thomas J M. Chem Mater, 1996, 8: 1112[18] Lewis D W, Catlow C R A, Thomas J M. Chem Mater, 1996, 8: 1112
19. [19] Muncaster G, Davies A T, Sankar G, Catlow C R A, Thomas J M, Colston S L, Barnes P, Walton R I, O'Hare D. Phys Chem Chem Phys, 2000, 2: 3523[19] Muncaster G, Davies A T, Sankar G, Catlow C R A, Thomas J M, Colston S L, Barnes P, Walton R I, O'Hare D. Phys Chem Chem Phys, 2000, 2: 3523
20. [20] Rey F, Sankar G, Thomas J M, Barrett P A, Lewis D W, Catlow C R A, Clark S M, Greaves G N. Chem Mater, 1995, 7: 1435[20] Rey F, Sankar G, Thomas J M, Barrett P A, Lewis D W, Catlow C R A, Clark S M, Greaves G N. Chem Mater, 1995, 7: 1435
21. [21] Sanchez-Sanchez M, Sankar G, Simperler A, Bell R G, Catlow C R A, Thomas J M. Catal Lett, 2003, 88: 163[21] Sanchez-Sanchez M, Sankar G, Simperler A, Bell R G, Catlow C R A, Thomas J M. Catal Lett, 2003, 88: 163
22. [22] Sankar G, Wyles J K, Catlow C R A. Top Catal, 2003, 24: 173[22] Sankar G, Wyles J K, Catlow C R A. Top Catal, 2003, 24: 173
23. [23] Marchese L, Frache A, Gianotti E, Martra G, Causa M, Coluccia S. Microporous Mesoporous Mater, 1999, 30: 145[23] Marchese L, Frache A, Gianotti E, Martra G, Causa M, Coluccia S. Microporous Mesoporous Mater, 1999, 30: 145
24. [24] Briend M, Vomscheid R, Peltre M J, Man P P, Barthomeuf D. J Phys Chem, 1995, 99: 8270[24] Briend M, Vomscheid R, Peltre M J, Man P P, Barthomeuf D. J Phys Chem, 1995, 99: 8270
25. [25] Chen J S, Thomas J M, Sankar G. J Chem Soc, Faraday Trans, 1994, 90: 3455[25] Chen J S, Thomas J M, Sankar G. J Chem Soc, Faraday Trans, 1994, 90: 3455
26. [26] Chen J S, Thomas J M. J Chem Soc, Chem Commun, 1994: 603[26] Chen J S, Thomas J M. J Chem Soc, Chem Commun, 1994: 603
27. [27] Zenonos C, Sankar G, Cora F, Lewis D W, Pankhurst Q A, Catlow C R A, Thomas J M. Phys Chem Chem Phys, 2002, 4: 5421[27] Zenonos C, Sankar G, Cora F, Lewis D W, Pankhurst Q A, Catlow C R A, Thomas J M. Phys Chem Chem Phys, 2002, 4: 5421
28. [28] Sankar G, Wyles J K, Jones R H, Thomas J M, Catlow C R A, Lewis D W, Clegg W, Coles S J, Teat S J. Chem Commun, 1998: 117[28] Sankar G, Wyles J K, Jones R H, Thomas J M, Catlow C R A, Lewis D W, Clegg W, Coles S J, Teat S J. Chem Commun, 1998: 117
29. [29] Burton A, Darton R J, Davis M E, Hwang S J, Morris R E, Ogino I, Zones S I. J Phys Chem B, 2006, 110: 5273[29] Burton A, Darton R J, Davis M E, Hwang S J, Morris R E, Ogino I, Zones S I. J Phys Chem B, 2006, 110: 5273
30. [30] Catlow C R A, Ackermann L, Bell R G, Gay D H, Holt S, Lewis D W, Nygren M A, Sastre G, Sayle D C, Sinclair P E. J Mol Catal A, 1997, 115: 431[30] Catlow C R A, Ackermann L, Bell R G, Gay D H, Holt S, Lewis D W, Nygren M A, Sastre G, Sayle D C, Sinclair P E. J Mol Catal A, 1997, 115: 431
31. [31] Larson A C, Dreele R B V. GSAS Generalised Crystal Structure Analysis System. Los Alamos National Laboratory, Los Alamos, New Mexico, USA, 1997[31] Larson A C, Dreele R B V. GSAS Generalised Crystal Structure Analysis System. Los Alamos National Laboratory, Los Alamos, New Mexico, USA, 1997
32. [32] McCusker L B, Baerlocher C. Stud Surf Sci Catal, 2007, 168: 13[32] McCusker L B, Baerlocher C. Stud Surf Sci Catal, 2007, 168: 13
33. [33] McCusker L B, Von Dreele R B, Cox D E, Louer D, Scardi P. J Appl Crystallogr, 1999, 32: 36[33] McCusker L B, Von Dreele R B, Cox D E, Louer D, Scardi P. J Appl Crystallogr, 1999, 32: 36
34. [34] Freeman C M, Catlow C R A, Thomas J M, Brode S. Chem Phys Lett, 1991, 186: 137[34] Freeman C M, Catlow C R A, Thomas J M, Brode S. Chem Phys Lett, 1991, 186: 137
35. [35] Discover 3.1. Biosym Technologies Inc, San Diego, USA, 1996[35] Discover 3.1. Biosym Technologies Inc, San Diego, USA, 1996
36. [36] Maple J R, Dinur U, Hagler A T. Proc Natl Acad Sci U S A, 1988, 85: 5350[36] Maple J R, Dinur U, Hagler A T. Proc Natl Acad Sci U S A, 1988, 85: 5350
37. [37] Martis M, Smith A J, Tang C, Parker J E, Hyde T I, Watson M J, Baucherel X, Kohara S, Wakihara T, Sankar G. Phys Chem Chem Phys, 2013, 15: 11766 [38] Lewis D W, Freeman C M, Catlow C R A. J Phys Chem, 1995, 99: 11194[37] Martis M, Smith A J, Tang C, Parker J E, Hyde T I, Watson M J, Baucherel X, Kohara S, Wakihara T, Sankar G. Phys Chem Chem Phys, 2013, 15: 11766 [38] Lewis D W, Freeman C M, Catlow C R A. J Phys Chem, 1995, 99: 11194

扫一扫看文章

计量

PDF下载量: 0
文章访问数: 555
HTML全文浏览量: 7

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Location and orientation of the N,N-diisopropylethylamine template molecule in the AlPO₄-18 framework by X-ray synchrotron diffraction and molecular modelling

通讯作者: Gopinathan Sankar,Tel: +44-2076794664; E-mail: g.sankar@ucl.ac.uk

English

Location and orientation of the N,N-diisopropylethylamine template molecule in the AlPO₄-18 framework by X-ray synchrotron diffraction and molecular modelling

Corresponding author: Gopinathan Sankar,Tel: +44-2076794664; E-mail: g.sankar@ucl.ac.uk

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

计量

通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处